Light-Healable Supramolecular Nanocomposites Based on Modified Cellulose Nanocrystals

Polymers that can be repaired after being damaged are attractive, because this feature can improve the reliability, functionality, and lifetime of these materials. We report here light-healable nanocomposites based on a telechelic poly(ethylene-co-butylene) that was functionalized with hydrogen-bonding ureidopyrimidone (UPy) and cellulose nanocrystals (CNCs) decorated with the same binding motif. These nanocomposites show significantly improved mechanical properties when compared to the supramolecular polymer alone. When these materials are exposed to ultraviolet radiation, the UPy motifs are excited and the absorbed energy is converted into heat. This causes temporary disengagement of the hydrogen-bonding motifs, concomitant with a reversible decrease of the supramolecular polymers' molecular weight and viscosity. As a result, deliberately introduced defects can be healed quickly and efficiently, even at a filler content of 20% w/w, that is, in compositions that exhibit high strength and stiffness.